Method and apparatus for reducing iron ores by means of methane gas



March 20, 1956 H. GALLUSSER' 2,739,055

METHOD AND APPARATUS FOR REDUCING IRON ORES BY MEANS OF METHANE GAS Filed Jan. 29, 1953 5 Sheets-Sheet l INVENTOR Hans Gallusser.

BY wziy'mjf ATTORN E Y Mar 1956 H. GALLUSSER METHOD AND APPARATUS FOR REDUCING IRON ORES BY MEANS OF METHANE GAS 3 Sheets-Sheet 2 Filed Jan. 29, 1955 Ms Wz a G s m H ATTORNEY March 1956 H. GALLUSSER 2,739,055

METHOD AND APPARATUS FOR REDUCING IRON ORES BY MEANS OF METHANE GAS Filed Jan. 29, 1953 3 Sheets-Sheet 3 Q? m E Z:

3 X Aida 4/ K K\///////J 7//////M x A! K vw x1 x O METHOD AND APPARATUS FOR REDUCING IRON ORESBY MEANS OF METHANE GAS Hans Gallusser, Geneva, Switzerland, assigno'r to Atellers Des Charmilles S. A.,'Geneva, Switzerland, a company of Switzerland.

Application January 29, 1953, Serial No. 333,860 Claims priority, application Switzerland March 17, 1952 A 8 Claims. (Cl. 75-13) Various methods of reducing iron ores in a shaft or stack-type furnace by means of methane, in which the heat necessary for the reduction is supplied to the furnace from an outside source, are already known. Such a process, for example, is described in U. S. Patent No. 2,144,618. According to that process, cold methane is fed into the lower part of a shaft furnace. -In the lower hot zone of thefurnace, which is heated by electrical high-frequency means in the presence of metallic iron acting as a catalyst, the methane is decomposed into H2 and C. The carbon is deposited on. the iron, whereas the hydrogen flows farther upward in the furnace where it. reduces the iron oresto'iron. a

Furthermore, methane is introduced through the upper part of the furnace and conducted-as far as the lower part of the zone which is heated by the high-frequency means. the reduced ore and decomposed into H2 and C through theeffect. of the iron as a catalyst,*whereupon the H2 flows upward through the furnace body while the carbon precipitates on the iron.

In practice, the process outlined above has the following disadvantages:

- 1(1)v The separated carbon is" not used for reduction,

which means a loss in efiicien'cy.

(2) Only about /3 of thehydrogen formed is capable of reduction, because chemical equilibrium occurs as soon as /2. of the hydrogen has been converted into water vapor as a result of reduction at a reduction temperature of 800-1000C., so that there can be no further'reduction. The other of the hydrogen formed leaves the furnace without participating in the reduction.

(3) The furnace is heated by electrical high-frequency means. Such heating is extremely uneconomical inasmuch as the standard electric energy of 50 to 60 cycles must be transformed into energy of 5,00010,000 cycles. This type of heating, moreover, is of low efliciency.

The general object of the present invention is the utilization of both components of the methane, namely, C and Hz, for reduction purposes and is based on the principle that, at high temperatures, methane is decom posed by water vapor into CO and H2 in accordance with the equation CH4+H2O=CO+3H2-49 K cal., both of these gases being excellent reducing gases for changing oxide into iron. 7

According to the present invention, the methane or the methane-containing gases as well as the ore to .be reduced, are heated together in a shaft furnace in known manner by a special heating system to the decomposition or reduction temperature. However, the process of the present invention differs from the known processes in that the waste gases, freed from water vapor and CO2, are again supplied alone into the furnace below the reduction zone and the methane or the methane-containing gases are fed through a special conduit into the upper part ofthe reduction zone of the furnace where they mix with the water vapor which has formed in the 'lower reduction zone through the reduction of the iron ore by hydrogen.

, water-vapor can no longer form, with the result that the V 2 The aforementioned cleansed waste gases will hereinafter he referred to as circulating gases.

In prior processes, the separation of carbon in the lower part of the furnace is due to the fact that the methane is fed into that part of the furnace where the iron oxides have already been reduced to iron so that methaneis decomposed into H2 and C under the influence of the high temperature. 7

According to the present invention, the separation of carbon is prevented by the fact that, through a special conduit and preferably at a high rate of speed, the methane is supplied into the upper part of the reduction zone which is heated by the aforementioned special heating system and where, and only then, it is mixed with the circulating gas which already contains suflicient Water vapor that has formed. through reduction in the lower part of the reduction zone. The accompanying drawings show diagrammatically and by way of example some embodiments of apparatus designed to carry the process into practice. Figure 1 is a diagrammatic sketch of a typical installation. I 'Figure 2 is a longitudinal section through an electric furnace. j

Figure 3 is a section along line III--III of Figure 2. Figure 4 is a longitudinal section through afurnace I heated by gas supplied from the outside.

There, the methane is brought into contact with circulating gases.

Figures 5 and 6 are enlarged detail tary portions. v i In Figure 1, the furnaceibody of a shaft furnace 10 is views of fragmenshown diagrammatically, the mid-section'of the furnace 1 being provided with a special heating system by means' of which the heat necessary for attaining the decomposition or reduction temperature of 800ff-1000" C. is pro:

duced and keptconstant. The'furnace has three principal zones, as shown in Figure 1, namely, the lower zone a, the middle or heating zone b, and the lower zone 0. Reduction of the iron ores takes place in zone b and will, therefore; hereinafter .be referred to as the reduction zone. The heating system may be either of the electric resistance orinduction heating or gas heating type.

Above and below the reduction zone b are substantially large spaces 14 and 15 respectively. In space 14 the hot gases heat the incoming cold ores, whereas in space 15 the hot reduced ores are cooled by the infiowing cold Spaces 14 and 15 are in communication with inlet and discharge arrangements (not shown) for the ores, but which are well known to the art.

The drawing shows diagrammatically how the methane or the 1nethanecontaining gases are fed into the furnace with a view to preventing the separation of carbon.

The methane or the methane-containing gases are introduced into the upper part of the reduction zone b by meansof a conduit 16 extending through the upper part or zonec of the furnace. This may extend, alternatively,

' laterally into the heating zone b, as shown on the drawmoval, by suction, of the waste gases. After treatment,

for the purpose of removing the Water vapor and the CO2, the remaining H2 and CO gases, hereinafter termed circulating gases, are fed again or recycled into the lower part 15 of the furnace through an inlet conduit 17.

The furnace operates as follows:

The cold circulating gas, consisting of Hz and CO, is warmed in the lower zone a by the reduced hot ores coming from the reduction zone b, as a result of which the ores are correspondingly cooled. Reduction of the iron ores begins in the lower part of the zone b jointly with the formation of water vapor and 7 139,055 i Patented Mar. 20, d

amass-a C02. The methane must now enter thereduction -zoneb at that place where there is already sufficient water vapor in the circulating gas to decompose the incoming methane into-CO and H2. Thesenewlyformed gases participate in the reductionuntil chemical equilibrium is'esta'b lished between Hzj' HzO,COand'CO2. Before leaving the furnace, these gases" heat theincoming' ores and are correspondingiy cooled ingiving up their heat for thispurp ose The ieduction'gasesare sucked from the upper part 14 of the furnace by a compressor '41 through conduit 18 and passed into a cooler'42, whereby the water formed by the reduction is condensed. Followingseparation of the water," the gases treated inknown fnanner ina washing pla'ntA for the purpose of removing the existing CO2 and thereby con'ceiitrating the H and CO. The remaining cold gases Hz and-cfiinthefpurified state are recycled int o the lower partl5'of the furnace through the conduit 17 By this method it ispos'sible" to use for reduction not only the h'ydrognof the"methane but also the carbon in the" form ofCO, inasmuch as the carbon is converted into C9 by the water vapor as a result of reduction with hydrogen.

In Figures 2"and 3, the body of the shaft furnace 10 is provided with an electrical induction heating system comprising astahdard transformerwith closed iron core built into the furnace. The numeral 7 designates the magnet frame'and '8 the primary windings of a 3-phase transformer.

it The three arms 12 of themagnet frame extend through the furnace body within adequately large ducts so that an air gap 9 remains between the windings S and the furnace body. As apparent from the drawing, those parts of the furnace body which are traversed by the arms 12 of the transformer are each surrounded by an insulated metal cylinder 11. These cylinders form the secondary windings of the transformer.

, A ventilatoror fan 1;: is provided at one end of each enveloped arm 12. Through airgap 9this ventilator removes the heat generated by the primary windings 8 as well as the heat flowing from the secondary windings ll-inward.

In all other respects, the arrangement of the installation is the same as that described in connection with Figure l. 'lts'mode of operation is'also the same.

This heating system isfar more efiicient than highfrequency heating. The degree of efficiency of a transformerof 'the type described amounts to about 97'percent where the cosine of the'phase angle between voltage and current, or power factor, lies between 0;85 and 0.9. This type of heating with standard electric energy of to cycles affords maximumbeating'effect.

Where an'inexpensive' heating 'gas,such' as natural gas or coke-oven gas, for instance, is available, the reduction furnace may be supplied with the necessary heat also from an outside source through the combustion of'such gases. An example of an installation of this type is shown in Figs. 4 to 6. v

In this case, the furnace body 10 comprises a material possessing-high insulating properties in order to keep the heatlosses of the furnace down to a minimum. The inner furnace wall comprises a heat-resisting metal cylinder 20, a portion of the length of which is surrounded by a gas heating system. This heating system comprises a tier of annular mutually connected ducts 21 which are in communication with a gas inlet 22 and a gas outlet 23 for hot combustion gases. The heating system may comprisebricks 24 of material having high heat conductive properties such asmagnesite bricks, forinstance, to transmit and give off to'the adjoining walls of the cylinilerifi the heat produced by the combustion of the gas and, at the same tinteyrirbtectthat wall against attack by combustiongases. I shown in Figures 5a nd6," each of the superposed annular ducts 21is'sealed at one point by a wall or ba fiie 25,whcreas"anaperture'l finext'tothat wall connects the duct with the ducts directly above and underneath it, so

that the heating gases fed into the lowermost duct must succesisvely flow through all annular ducts.

Ducts 21 may also be slightly inclined and form a spiral or helical pattern"between gas inlet 22 and gas outlet 23.

l. The method of reducing iron oxide in avertical stack type furnace, consisting essentially of electrically heating the iron oxide in the presence'of substantially pure hydrogen and substantially pure carbon monoxide at a reduction temperature in an intermediate part of said furnace, reacting gases evolving from the reduction reaction," which gases will include steam asa product 'of the reduction of iron-oxide withhydrogen, with methane gas to form hydrogen and carbon monoxide, said methane gas being introduced inthe upper part of said intermediate part of said furnace, purifyingjth'e evolving gas'es'to'cbncentrate the hydrogen and carbon monoxide content thereof, and recycling the purified gas alone for reaction with the" iron oxide,belo'w said intermediatepart.

'2. The method'of reducing iron oxide in a vertical stack type furnace,consisting essentially of electrically heating the iron oxide' in the presence ofsubstaritially purehydrogen and substantially pure carbon monoxideat a reduction temperature in an intermediate part of said furnace, reacting gases evolving from the reduction reactionywhicihflgaseswill includesteam as a product-of the reductionof 'irdn' oxide' with hydrogen admixed with c'arbon dioxide, with methanegas to form hydrogenand carb n nidnoTdepsaid"methane gas being introduced in upper part of said intermediate part of said furnace, removing carbon dioxide and water from the resulting gaseons mixture] and recycling'it alone for reaction with the iron'oxide, below said ntermediate part.

3. Thernethddof reducing iron oxide in a vertical stacktype furnace, "consisting essentially of electrically heating the iron oxide in the presenceofsubstantially'pure hydrogen "and substantially pure carbon monoxide at a temperature in the range of about 800 to'1000 C., in an" intermediate part of said furnace; reacting g'ase's evolving from v the reduction reactionfwhich gaseswill include steam asf-a"product' of the reduction of iron oxide with hydrogen admixedwith carbon dioxide, with methane gas to form hydrogenand carbori'monoxide, said methane gas being" introduced in the upper part'ofsaid intermediate part of said furnace,ren1oving carbon dioxide and water from measuring gaseous mixture and recycling it alone for reactionwiththe iron oxide, below said intermediate P l 4. "pparatns' for reducing iron oxide comprising'a ver tical'fstack'type furnace having an upper zone, a lower zone and an intermediate zone, said zones being adapted to be chargedwith iron oxide to be reduced, meansfor electrically heating said intermediate zone to the reduction temperature, said furnace having a'first gas inlet leading to'the upper part of said intermediate zone, said inlet being adapted toconduct methane gas to the furnacefroin an external source'of supply,a' gas outlet at the top of said upper zone and above said first gas inlet, a second gas inlet at the'bottom of said lower zone, and a gas pump and gas purification means connected betweeen' said outlet and said second' gas inlet, said means being operative to continuously peacetime hydrogen and carbon monoxide component's ot' a; gaseous medium containing said conielectrically "heating an intermediatejzone m there'duction temperature, furnace having a first gas: inlet leading to'tlie'uppe'r' t of said intermediate zonefs aid inletb 'g upper zone and above said first gas inlet, a second gas inlet at the bottom of said lower zone, means for pumping gases from said outlet to saId second inlet, and means for removing carbon dioxide and water from said pumped gases before re-entering the furnace through said second gas inlet.

6. Apparatus as defined by claim 5 in which the heating means is of the electrical induction type and having a transformer, said transformer having a closed iron core within the furnace and having its secondary winding integral with the wall of the furnace.

7. Apparatus as defined by claim 5 in which the heating means comprises a tier of ducts surrounding the wall of the furnace, and means for serially conducting hot gases through said ducts.

8. The method of reducing iron'oxide in a stack type furnace, said method consisting essentially of electrically heating an intermediate zone of the furnace to a temperature of about 800 to 1000 C., passing iron oxide to be reduced from an upper zone of the furnace downwardly through the intermediate zone and thence passing iron reduced in the intermediate zone through a bottom zone of the furnace, passing upwardly through the bot-tom zone a cold gaseous mixture of substantially pure hydrogen and substantially pure carbon monoxide, whereby the reduced iron is cooled by the gaseous mixture and the gaseous mixture is heated WithObt substantial chemical change therein, passing the hot gaseous mixture upwardly through the intermediate zone to react with the heated oxide and effect reduction thereof with formation of water and carbon dioxide, introducing methane gas into the upper part of the intermediate zone to react with a portion of the formed water and carbon dioxide to form hydrogen and carbon monoxide, removing excess water, carbon dioxide,

' hydrogen and carbon monoxide as a gaseous mixture from the top of the intermediate zone, treating the removed gaseous mixture to eliminate water and carbon dioxide, said treatment including cooling, whereby a cold mixture of substantially pure hydrogen and substantially pure car bon monoxide obtains, and recycling the latter cold mixture by introducing it at the bottom of the lower zone of the furnace.

References Cited in the file of this patent UNITED STATES PATENTS 

1. THE METHOD OF REDUCING IRON OXIDE IN A VERTICAL STACK TYPE FURNACE, CONSISTING ESSENTIALLY OF ELECTRICALLY HEATING THE IRON OXIDE IN THE PRESENCE OF SUBSTANTIALLY PURE HYDROGEN AND SUBSTANTIALLY PURE CARBON MONOXIDE AT A REDUCTION TEMPERATURE IN AN INTERMEDIATE PART OF SAID FURNACE, REACTING GASES EVOLVING FROM THE REDUCTION REACTION, WHICH GASES WILL INCLUDE STEAM AS A PRODUCT OF THE REDUCTION OF IRON OXIDE WITH HYDROGEN, WITH METHANE GAS TO FORM HYDROGEN AND CARBON MONOXIDE, SAID METHANE GAS BEING INTRODUCED IN THE UPPER PART OF SAID INTERMEDIATE PART OF SAID FURNACE, PURIFYING THE EVOLVING GASES TO COMCENTRATE AND HYDROGEN AND CARBON MONOXIDE CONTENT THEREOF, AND RECYCLING THE PURIFIED GAS ALONE FOR REACTION WITH THE IRON OXIDE, BELOW SAID INTERMEDIATE PART. 